The rapid changes in the pattern of atmospheric warming as well as the degradation of glaciers in the Himalayas point to the inevitability of accurate source characterization and quantification of the impact of aerosols. In this regard, optical and chemical properties of aerosols, and their role in radiative effects are examined over a remote high-altitude site Lachung (27.4 degrees N, 88.4 degrees E, 2700 m a.s.l.) in the eastern Himalayas during August-2018 to February-2020. It is found that the sulphate (SO42- ) and carbonaceous aerosols (both organic carbon - OC and elemental carbon - EC) significantly contribute to the total aerosol mass loading in winter (DJF) and spring (MAM), resulting in high values of scattering and absorption coefficients. Aerosol single scattering albedo (SSA) is relatively higher in winter ( 0.85) due to a significantly higher amount of OC (OC/EC > 8). However, SSA 0.8 in spring despite of higher SO42- concentrations (SO42- /EC > 4.0 and SO42-/OC - 1.0) than winter. A reverse pattern is seen in summer-monsoon (JJAS) having lower SO42-/EC < 2 and SO42- /OC < 0.5, resulting in SSA as low as -0.64. The seasonal values of aerosol direct radiative forcing in the top of the atmosphere (DRFTOA) are as high as -2.9 +/- 1.2 Wm- 2 during the period of abundant OC in winter and -2.8 +/- 0.5 Wm- 2 during the period of abundant SO42- in spring. The combined effect of carbonaceous and SO42- aerosols on the surface cooling is highest in spring (-16.7 +/- 4.9 Wm- 2). DRF in the atmosphere is also - 34% higher in spring (13.8 +/- 4.5 Wm- 2, which translates to an atmospheric heating rate of - 0.39 K day-1), than in winter. The seasonal pattern of forcing influenced by the heterogeneous sources and chemical composition of aerosols over the eastern Himalayan site is significantly influenced by the transport of aerosols from the Indo-Gangetic Plains of India.

Three global chemistry-transport models (CTM) are used to quantify the radiative forcing (RF) from aviation NOx emissions, and the resultant reductions in RF from coupling NOx to aerosols via heterogeneous chemistry. One of the models calculates the changes due to aviation black carbon (BC) and sulphate aerosols and their direct RF, as well as the BC indirect effect on cirrus cloudiness. The surface area density of sulphate aerosols is then passed to the other models to compare the resulting photochemical perturbations on NOx through heterogeneous chemical reactions. The perturbation on O-3 and CH4 (via OH) is finally evaluated, considering both short- and long-term O-3 responses. Ozone RF is calculated using the monthly averaged output of the three CTMs in two independent radiative transfer codes. According to the models, column ozone and CH4 lifetime changes due to coupled NOx/aerosol emissions are, on average, +0.56 Dobson Units (DU) and -1.1 months, respectively, for atmospheric conditions and aviation emissions representative of the year 2006, with an RF of +16.4 and -10.2 mW/m(2) for O-3 and CH4, respectively. Sulphate aerosol induced changes on ozone column and CH4 lifetime account for -0.028 DU and +0.04 months, respectively, with corresponding RFs of -0.63 and +0.36 mW/m(2). Soot-cirrus forcing is calculated to be 4.9 mW/m(2).

A box model has been used to compare the burdens, optical depths and direct radiative forcing from anthropogenic PM2.5 aerosol constituents over the Indian subcontinent. A PM2.5 emission inventory from India for 1990, compiled for the first time, placed anthropogenic aerosol emissions at 12.6 Tg yr(-1). The contribution from various aerosol constituents was 28% sulphate, 25% mineral (clay), 23% fly-ash, 20% organic matter and 4% black carbon. Fossil fuel combustion and biomass burning accounted for 68% and 32%, respectively, of the combustion aerosol emissions. The monthly mean aerosol burdens ranged from 4.9 to 54.4 mg m(-2) with an annual average of 18.4 +/- 22.1 mg m(-2). The largest contribution was from fly-ash from burning of coal (40%), which has a high average ash content of 30%. This was followed by contributions of organic matter (23 %) and sulphate (22%). Alkaline constituents of fly-ash could neutralise rainfall acidity and contribute to the observed high rainfall alkalinity in this region. The estimated annual average optical depth was 0.08 +/- 0.06, with sulphate accounting For 36%, organic matter for 32% and black carbon for 13%, in general agreement with those of Satheesh et al. (1999). The mineral aerosol contribution (5%) was lower than that from the previous study because of wet deposition from high rainfall in the months of high emissions and the complete mixing assumption in the box model. The annual average radiative forcing was - 1.73 +/- 1.93 W m-2 with contributions of 49% from sulphate aerosols, followed by organic matter (26%), black carbon (11%) and fly-ash (11%). These results indicate the importance of organic matter and fly-ash to atmospheric optical and radiative effects. The uncertainties in estimated parameters range 80-120% and result largely from uncertainties in emission and wet deposition rates. Therefore, improvement is required in the emissions estimates and scavenging ratios, to increase confidence in these predictions. (C) 2000 Elsevier Science Ltd. All rights reserved.